Electrochemical phenomena occur on vastly different time and length scales, yet the performance of an electrochemical cell is determined by the highly coupled behavior of these phenomena. Computational simulations have been traditionally used to study these different physical scales in isolation. The latest work in our group seeks to unify phenomena from the atomistic to continuum levels through the development of multi-scale computational models. Work in recent years utilizing such an approach has shown better prediction and determination of experimental work [1].

Due to the rapid rate with which we must develop, scale-up, and deploy decarbonization technologies, or group is particularly focused on applying multi-scale methods to integrated carbon capture and conversion systems. Our work utilizes state of the art atomistic approaches such as grand canonical density functional theory calculations in concert with microkinetic modeling and one- to three-dimensional transport models [2 - 4]. Through close collaborations with experimentalists utilizing techniques such as operando spectroscopy, we are developing a robust feedback loop that will provide a detailed picture of the reaction environment for CO₂from the moment it enters our system to its exit.

Our models can determine species coverages, concentration and potential profiles, mechanistic pathways, pH regimes, electrolyte effects, and other parameters related to real-world operating conditions. Through such data, we can design better, more efficient catalysts and electrochemical cells. This talk will focus on the applications of such a multi-scale model to electrochemical CO₂ conversion over a baseline catalyst and its implications for an integrated, reactive capture system that captures atmospheric CO₂ and yields a reduced product.

References:

[1] PNAS October 17, 2017 114 (42) E8812-E8821

[2] J. Phys. Chem. C, 2021, 125, 43, 23773–23783

[3] Energy Environ. Sci., 2019, 12, 3380

[4] ACS Sustainable Chem. Eng. 2021, 9, 3, 1286–1296